TY - JOUR
T1 - Design of stable mixed-metal MIL-101(Cr/Fe) materials with enhanced catalytic activity for the Prins reaction
AU - Vallés-García, Cristina
AU - Gkaniatsou, Effrosyni
AU - Santiago-Portillo, Andrea
AU - Giménez-Marqués, Mónica
AU - Álvaro, Mercedes
AU - Greneche, Jean Marc
AU - Steunou, Nathalie
AU - Sicard, Clémence
AU - Navalón, Sergio
AU - Serre, Christian
AU - García, Hermenegildo
N1 - Funding Information:
Financial support by the Spanish Ministry of Economy and Competitiveness (Severo Ochoa, CTQ2018-890237-CO2-R1 and Maria de Maeztu, CEX2019-000919-M), is gratefully acknowledged. Generalidad Valenciana is also thanked for funding (Prometeo 2017/083). S. N. thanks nancial support by the Min-isterio de Ciencia, Innovación y Universidades (RTI 2018-099482-A-I00 project), Fundación Ramón Areces (XVIII Concurso Nacio-nal para la Adjudicación de Ayudas a la Investigación en Ciencias de la Vida y de la Materia, 2016), and Generalitat Valenciana grupos de investigación consolidables 2019 (ref: AICO/2019/214) project. E. G. thanks the ANR-11-LABEX-0039 (LabEx CHARM3AT) for nancial support. M. G.-M thanks support from “la Caixa” Foundation (LCF/BQ/PI19/11690022) and Generalitat Valenciana (SEJI/2020/036).
Publisher Copyright:
© 2020 The Royal Society of Chemistry.
Copyright:
Copyright 2020 Elsevier B.V., All rights reserved.
PY - 2020/9/7
Y1 - 2020/9/7
N2 - This work highlights the benefit of designing mixed-metal (Cr/Fe) MOFs for enhanced chemical stability and catalytic activity. A robust and stable mixed-metal MIL-101(Cr/Fe) was prepared through a HF-free direct hydrothermal route with Fe3+ content up to 21 wt%. The incorporation of Fe3+ cations in the crystal structure was confirmed by 57Fe Mössbauer spectrometry. The catalytic performance of the mixed metal MIL-101(Cr/Fe) was evaluated in the Prins reaction. MIL-101(Cr/Fe) exhibited a higher catalytic activity compared to MIL-101(Cr), improved chemical stability compared to MIL-101(Fe) and a higher catalytic activity for bulky substrates compared to MIL-100(Fe). In situ infra-red spectroscopy study suggests that the incorporation of Fe3+ ions in MIL-101 structure leads to an increase in Lewis acid sites. It was thus concluded that the predominant role of Cr3+ ions was to maintain the crystal structure, while Fe3+ ions enhanced the catalytic activity.
AB - This work highlights the benefit of designing mixed-metal (Cr/Fe) MOFs for enhanced chemical stability and catalytic activity. A robust and stable mixed-metal MIL-101(Cr/Fe) was prepared through a HF-free direct hydrothermal route with Fe3+ content up to 21 wt%. The incorporation of Fe3+ cations in the crystal structure was confirmed by 57Fe Mössbauer spectrometry. The catalytic performance of the mixed metal MIL-101(Cr/Fe) was evaluated in the Prins reaction. MIL-101(Cr/Fe) exhibited a higher catalytic activity compared to MIL-101(Cr), improved chemical stability compared to MIL-101(Fe) and a higher catalytic activity for bulky substrates compared to MIL-100(Fe). In situ infra-red spectroscopy study suggests that the incorporation of Fe3+ ions in MIL-101 structure leads to an increase in Lewis acid sites. It was thus concluded that the predominant role of Cr3+ ions was to maintain the crystal structure, while Fe3+ ions enhanced the catalytic activity.
UR - http://www.scopus.com/inward/record.url?scp=85090587338&partnerID=8YFLogxK
U2 - 10.1039/d0ta02991b
DO - 10.1039/d0ta02991b
M3 - Article
AN - SCOPUS:85090587338
VL - 8
SP - 17002
EP - 17011
JO - Journal of Materials Chemistry A
JF - Journal of Materials Chemistry A
SN - 2050-7488
IS - 33
ER -
